Forward flux sampling calculation of homogeneous nucleation rates from aqueous NaCl solutions

Jiang, Hao; Haji-Akbari, Amir; Debenedetti, Pablo G.; Panagiotopoulos, Athanassios Z.

doi:10.1063/1.5016554

Title: Forward flux sampling calculation of homogeneous nucleation rates from aqueous NaCl solutions

Journal Article · Thu Jan 25 00:00:00 EST 2018 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.5016554· OSTI ID:1512939

^[1];

^[2];

^[1];

^[1]

Princeton Univ., NJ (United States). Dept. of Chemical and Biological Engineering
Yale Univ., New Haven, CT (United States). Dept. of Chemical and Environmental Engineering

We used molecular dynamics simulations and the path sampling technique known as forward flux sampling to study homogeneous nucleation of NaCl crystals from supersaturated aqueous solutions at 298 K and 1 bar. Nucleation rates were obtained for a range of salt concentrations for the Joung-Cheatham NaCl force field combined with the Extended Simple Point Charge (SPC/E) water model. The calculated nucleation rates are significantly lower than the available experimental measurements. The estimates for the nucleation rates in this work do not rely on classical nucleation theory, but the pathways observed in the simulations suggest that the nucleation process is better described by classical nucleation theory than an alternative interpretation based on Ostwald’s step rule, in contrast to some prior simulations of related models. In addition to the size of NaCl nucleus, we find that the crystallinity of a nascent cluster plays an important role in the nucleation process. Nuclei with high crystallinity were found to have higher growth probability and longer lifetimes, possibly because they are less exposed to hydration water.

View Accepted Manuscript (DOE)

View Accepted Manuscript (Publisher)

Cite

Export

Save

Research Organization:: Princeton Univ., NJ (United States)

Sponsoring Organization:: USDOE; National Science Foundation (NSF)

Grant/Contract Number:: SC0002128; TG-CHE170059

OSTI ID:: 1512939

Alternate ID(s):: OSTI ID: 1418078

Journal Information:: Journal of Chemical Physics, Vol. 148, Issue 4; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

Citation Metrics:

Cited by: 44 works

Citation information provided by
Web of Science

References (58)

Consensus on the solubility of NaCl in water from computer simulations using the chemical potential route Benavides, A. L.; Aragones, J. L.; Vega, C. The Journal of Chemical Physics, Vol. 144, Issue 12 https://doi.org/10.1063/1.4943780	journal	March 2016
Forward flux sampling for rare event simulations Allen, Rosalind J.; Valeriani, Chantal; Rein ten Wolde, Pieter Journal of Physics: Condensed Matter, Vol. 21, Issue 46 https://doi.org/10.1088/0953-8984/21/46/463102	journal	October 2009
Molecular dynamics simulation in the grand canonical ensemble Eslami, Hossein; Müller-Plathe, Florian Journal of Computational Chemistry, Vol. 28, Issue 10 https://doi.org/10.1002/jcc.20689	journal	January 2007
Nucleation of NaCl from Aqueous Solution: Critical Sizes, Ion-Attachment Kinetics, and Rates Zimmermann, Nils E. R.; Vorselaars, Bart; Quigley, David Journal of the American Chemical Society, Vol. 137, Issue 41 https://doi.org/10.1021/jacs.5b08098	journal	October 2015
Pharmaceutical Crystallization Chen, Jie; Sarma, Bipul; Evans, James M. B. Crystal Growth & Design, Vol. 11, Issue 4 https://doi.org/10.1021/cg101556s	journal	April 2011
Crystal nucleation of hard spheres using molecular dynamics, umbrella sampling, and forward flux sampling: A comparison of simulation techniques Filion, L.; Hermes, M.; Ni, R. The Journal of Chemical Physics, Vol. 133, Issue 24 https://doi.org/10.1063/1.3506838	journal	December 2010
Sampling Rare Switching Events in Biochemical Networks Allen, Rosalind J.; Warren, Patrick B.; ten Wolde, Pieter Rein Physical Review Letters, Vol. 94, Issue 1 https://doi.org/10.1103/physrevlett.94.018104	journal	January 2005
Molecular simulation of thermodynamic and transport properties for the H ₂ O+NaCl system Orozco, Gustavo A.; Moultos, Othonas A.; Jiang, Hao The Journal of Chemical Physics, Vol. 141, Issue 23 https://doi.org/10.1063/1.4903928	journal	December 2014
Computational investigation of structure, dynamics and nucleation kinetics of a family of modified Stillinger–Weber model fluids in bulk and free-standing thin films Gianetti, Melisa M.; Haji-Akbari, Amir; Paula Longinotti, M. Physical Chemistry Chemical Physics, Vol. 18, Issue 5 https://doi.org/10.1039/c5cp06535f	journal	January 2016
Metastability Limit for the Nucleation of NaCl Crystals in Confinement Desarnaud, Julie; Derluyn, Hannelore; Carmeliet, Jan The Journal of Physical Chemistry Letters, Vol. 5, Issue 5 https://doi.org/10.1021/jz500090x	journal	February 2014
New Perspectives on Mineral Nucleation and Growth: From Solution Precursors to Solid Materials Van Driessche, Alexander E. S.; Kellermeier, Matthias; Benning, Liane G. https://doi.org/10.1007/978-3-319-45669-0	book	January 2017
GROMACS: Fast, flexible, and free Van Der Spoel, David; Lindahl, Erik; Hess, Berk Journal of Computational Chemistry, Vol. 26, Issue 16 https://doi.org/10.1002/jcc.20291	journal	January 2005
Molecular Simulations of Aqueous Electrolyte Solubility: 1. The Expanded-Ensemble Osmotic Molecular Dynamics Method for the Solution Phase Lísal, Martin; Smith, William R.; Kolafa, Jiří The Journal of Physical Chemistry B, Vol. 109, Issue 26 https://doi.org/10.1021/jp0507492	journal	July 2005
Rate of homogeneous crystal nucleation in molten NaCl Valeriani, C.; Sanz, E.; Frenkel, D. The Journal of Chemical Physics, Vol. 122, Issue 19 https://doi.org/10.1063/1.1896348	journal	May 2005
Ion-Induced Nucleation in Solution : Promotion of Solute Nucleation in Charged Levitated Droplets Draper, Neil D.; Bakhoum, Samuel F.; Haddrell, Allen E. Journal of the American Chemical Society, Vol. 129, Issue 37 https://doi.org/10.1021/ja067094i	journal	September 2007
Recent progress in molecular simulation of aqueous electrolytes: force fields, chemical potentials and solubility Nezbeda, Ivo; Moučka, Filip; Smith, William R. Molecular Physics, Vol. 114, Issue 11 https://doi.org/10.1080/00268976.2016.1165296	journal	March 2016
Forward flux sampling-type schemes for simulating rare events: Efficiency analysis Allen, Rosalind J.; Frenkel, Daan; ten Wolde, Pieter Rein The Journal of Chemical Physics, Vol. 124, Issue 19 https://doi.org/10.1063/1.2198827	journal	May 2006
Atomistic Mechanism of NaCl Nucleation from an Aqueous Solution Zahn, Dirk Physical Review Letters, Vol. 92, Issue 4 https://doi.org/10.1103/physrevlett.92.040801	journal	January 2004
Direct calculation of ice homogeneous nucleation rate for a molecular model of water Haji-Akbari, Amir; Debenedetti, Pablo G. Proceedings of the National Academy of Sciences, Vol. 112, Issue 34 https://doi.org/10.1073/pnas.1509267112	journal	August 2015
Molecular Dynamics Simulations of the Dynamic and Energetic Properties of Alkali and Halide Ions Using Water-Model-Specific Ion Parameters Joung, In Suk; Cheatham, Thomas E. The Journal of Physical Chemistry B, Vol. 113, Issue 40 https://doi.org/10.1021/jp902584c	journal	October 2009
Efflorescence Relative Humidity of Mixed Sodium Chloride and Sodium Sulfate Particles Gao, Yonggang; Yu, Liya E.; Chen, Shing Bor The Journal of Physical Chemistry A, Vol. 111, Issue 42 https://doi.org/10.1021/jp073186y	journal	October 2007
Cluster formation in highly supersaturated solution droplets Na, Han-Soo; Arnold, Stephen; Myerson, Allan S. Journal of Crystal Growth, Vol. 139, Issue 1-2 https://doi.org/10.1016/0022-0248(94)90034-5	journal	May 1994
Chemical treatment technologies for waste-water recycling—an overview Gupta, Vinod Kumar; Ali, Imran; Saleh, Tawfik A. RSC Advances, Vol. 2, Issue 16 https://doi.org/10.1039/c2ra20340e	journal	January 2012
Solubility of NaCl in water by molecular simulation revisited Aragones, J. L.; Sanz, E.; Vega, C. The Journal of Chemical Physics, Vol. 136, Issue 24 https://doi.org/10.1063/1.4728163	journal	June 2012
PLUMED 2: New feathers for an old bird Tribello, Gareth A.; Bonomi, Massimiliano; Branduardi, Davide Computer Physics Communications, Vol. 185, Issue 2 https://doi.org/10.1016/j.cpc.2013.09.018	journal	February 2014
On the calculation of solubilities via direct coexistence simulations: Investigation of NaCl aqueous solutions and Lennard-Jones binary mixtures Espinosa, J. R.; Young, J. M.; Jiang, H. The Journal of Chemical Physics, Vol. 145, Issue 15 https://doi.org/10.1063/1.4964725	journal	October 2016
Thermodynamic and Transport Properties of H ₂ O + NaCl from Polarizable Force Fields Jiang, Hao; Mester, Zoltan; Moultos, Othonas A. Journal of Chemical Theory and Computation, Vol. 11, Issue 8 https://doi.org/10.1021/acs.jctc.5b00421	journal	July 2015
Crystal Nucleation in Liquids: Open Questions and Future Challenges in Molecular Dynamics Simulations Sosso, Gabriele C.; Chen, Ji; Cox, Stephen J. Chemical Reviews, Vol. 116, Issue 12 https://doi.org/10.1021/acs.chemrev.5b00744	journal	May 2016
How Crystals Nucleate and Grow in Aqueous NaCl Solution Chakraborty, Debashree; Patey, G. N. The Journal of Physical Chemistry Letters, Vol. 4, Issue 4 https://doi.org/10.1021/jz302065w	journal	January 2013
Temperature-dependent solubilities and mean ionic activity coefficients of alkali halides in water from molecular dynamics simulations Mester, Zoltan; Panagiotopoulos, Athanassios Z. The Journal of Chemical Physics, Vol. 143, Issue 4 https://doi.org/10.1063/1.4926840	journal	July 2015
Energy component analysis for dilute aqueous solutions of lithium(1+), sodium(1+), fluoride(1-), and chloride(1-) ions Chandrasekhar, Jayaraman; Spellmeyer, David C.; Jorgensen, William L. Journal of the American Chemical Society, Vol. 106, Issue 4 https://doi.org/10.1021/ja00316a012	journal	February 1984
Birth of NaCl Crystals: Insights from Molecular Simulations Lanaro, G.; Patey, G. N. The Journal of Physical Chemistry B, Vol. 120, Issue 34 https://doi.org/10.1021/acs.jpcb.6b05291	journal	August 2016
A molecular dynamics method for simulations in the canonical ensemble Nosé, Shūichi Molecular Physics, Vol. 52, Issue 2 https://doi.org/10.1080/00268978400101201	journal	June 1984
Heterogeneous Ice Nucleation Controlled by the Coupling of Surface Crystallinity and Surface Hydrophilicity Bi, Yuanfei; Cabriolu, Raffaela; Li, Tianshu The Journal of Physical Chemistry C, Vol. 120, Issue 3 https://doi.org/10.1021/acs.jpcc.5b09740	journal	January 2016
Surface-induced crystallization in supercooled tetrahedral liquids Li, Tianshu; Donadio, Davide; Ghiringhelli, Luca M. Nature Materials, Vol. 8, Issue 9 https://doi.org/10.1038/nmat2508	journal	August 2009
Particle mesh Ewald: An N ⋅log( N ) method for Ewald sums in large systems Darden, Tom; York, Darrin; Pedersen, Lee The Journal of Chemical Physics, Vol. 98, Issue 12 https://doi.org/10.1063/1.464397	journal	June 1993
The Ostwald step rule Van Santen, R. A. The Journal of Physical Chemistry, Vol. 88, Issue 24 https://doi.org/10.1021/j150668a002	journal	November 1984
Perspective: Surface freezing in water: A nexus of experiments and simulations Haji-Akbari, Amir; Debenedetti, Pablo G. The Journal of Chemical Physics, Vol. 147, Issue 6 https://doi.org/10.1063/1.4985879	journal	August 2017
Polymorphic transitions in single crystals: A new molecular dynamics method Parrinello, M.; Rahman, A. Journal of Applied Physics, Vol. 52, Issue 12 https://doi.org/10.1063/1.328693	journal	December 1981
Ion-water interaction potentials derived from free energy perturbation simulations Ȧqvist, Johan The Journal of Physical Chemistry, Vol. 94, Issue 21 https://doi.org/10.1021/j100384a009	journal	October 1990
Computational investigation of surface freezing in a molecular model of water Haji-Akbari, Amir; Debenedetti, Pablo G. Proceedings of the National Academy of Sciences, Vol. 114, Issue 13 https://doi.org/10.1073/pnas.1620999114	journal	March 2017
Salt Crystallization from an Evaporating Aqueous Solution by Molecular Dynamics Simulations Mucha, Martin; Jungwirth, Pavel The Journal of Physical Chemistry B, Vol. 107, Issue 33 https://doi.org/10.1021/jp034461t	journal	August 2003
Ions in water: From ion clustering to crystal nucleation Alejandre, José; Hansen, Jean-Pierre Physical Review E, Vol. 76, Issue 6 https://doi.org/10.1103/physreve.76.061505	journal	December 2007
Thermodynamics of electrolytes. IV. Activity and osmotic coefficients for mixed electrolytes Pitzer, Kenneth S.; Kim, Janice J. Journal of the American Chemical Society, Vol. 96, Issue 18 https://doi.org/10.1021/ja00825a004	journal	September 1974
Simultaneous estimation of free energies and rates using forward flux sampling and mean first passage times Thapar, Vikram; Escobedo, Fernando A. The Journal of Chemical Physics, Vol. 143, Issue 24 https://doi.org/10.1063/1.4938248	journal	December 2015
The missing term in effective pair potentials Berendsen, H. J. C.; Grigera, J. R.; Straatsma, T. P. The Journal of Physical Chemistry, Vol. 91, Issue 24 https://doi.org/10.1021/j100308a038	journal	November 1987
Probing Methane Hydrate Nucleation through the Forward Flux Sampling Method Bi, Yuanfei; Li, Tianshu The Journal of Physical Chemistry B, Vol. 118, Issue 47 https://doi.org/10.1021/jp503000u	journal	June 2014
Evidence that crystal nucleation in aqueous NaCl solution Occurs by the two-step mechanism Chakraborty, Debashree; Patey, G. N. Chemical Physics Letters, Vol. 587 https://doi.org/10.1016/j.cplett.2013.09.054	journal	November 2013
Transient Polymorphism in NaCl Giberti, Federico; Tribello, Gareth A.; Parrinello, Michele Journal of Chemical Theory and Computation, Vol. 9, Issue 6 https://doi.org/10.1021/ct4002027	journal	May 2013
LINCS: A linear constraint solver for molecular simulations Hess, Berk; Bekker, Henk; Berendsen, Herman J. C. Journal of Computational Chemistry, Vol. 18, Issue 12 https://doi.org/10.1002/(sici)1096-987x(199709)18:12<1463::aid-jcc4>3.0.co;2-h	journal	September 1997
Improving the specificity of organophosphorus hydrolase to acephate by mutagenesis at its binding site: a computational study Badakhshan, Reza; Mohammadi, Mozafar; Farnoosh, Gholamreza Journal of Molecular Modeling, Vol. 27, Issue 6 https://doi.org/10.1007/s00894-021-04749-6	journal	May 2021
A molecular dynamics method for simulations in the canonical ensemble NosÉ, SH[Ubar]ICHI Molecular Physics, Vol. 100, Issue 1 https://doi.org/10.1080/00268970110089108	journal	January 2002
Forward Flux Sampling for rare event simulations Allen, Rosalind J.; Valeriani, Chantal; Wolde, Pieter Rein ten arXiv https://doi.org/10.48550/arxiv.0906.4758	text	January 2009
Crystal nucleation of hard spheres using molecular dynamics, umbrella sampling and forward flux sampling: A comparison of simulation techniques Filion, Laura; Hermes, Michiel; Ni, Ran arXiv https://doi.org/10.48550/arxiv.1006.2925	text	January 2010
Direct Calculation of Ice Homogeneous Nucleation Rate for a Molecular Model of Water Haji-Akbari, Amir; Debenedetti, Pablo G. arXiv https://doi.org/10.48550/arxiv.1505.01126	text	January 2015
Computational investigation of structure, dynamics and nucleation kinetics of a family of modified Stillinger-Weber model fluids in bulk and free-standing thin films Gianetti, Melisa M.; Haji-Akbari, Amir; Longinotti, M. Paula arXiv https://doi.org/10.48550/arxiv.1510.07399	text	January 2015
Recent Progress in Molecular Simulation of Aqueous Electrolytes: Force Fields, Chemical Potentials and Solubility Nezbeda, Ivo; Moučka, Filip; Smith, William R. arXiv https://doi.org/10.48550/arxiv.1602.04065	text	January 2016
Perspective: Surface Freezing in Water: A Nexus of Experiments and Simulations Akbari, Amir Haji; Debenedetti, Pablo G. arXiv https://doi.org/10.48550/arxiv.1707.04797	text	January 2017

Cited By (6)

Calculation of critical nucleation rates by the persistent embryo method: application to quasi hard sphere models Ren, Shang; Sun, Yang; Zhang, Feng Soft Matter, Vol. 14, Issue 45 https://doi.org/10.1039/c8sm01415a	journal	January 2018
NaCl nucleation from brine in seeded simulations: Sources of uncertainty in rate estimates Zimmermann, Nils. E. R.; Vorselaars, Bart; Espinosa, Jorge R. The Journal of Chemical Physics, Vol. 148, Issue 22 https://doi.org/10.1063/1.5024009	journal	June 2018
Communication: Nucleation rates of supersaturated aqueous NaCl using a polarizable force field Jiang, Hao; Debenedetti, Pablo G.; Panagiotopoulos, Athanassios Z. The Journal of Chemical Physics, Vol. 149, Issue 14 https://doi.org/10.1063/1.5053652	journal	October 2018
Nucleation in aqueous NaCl solutions shifts from 1-step to 2-step mechanism on crossing the spinodal Jiang, Hao; Debenedetti, Pablo G.; Panagiotopoulos, Athanassios Z. The Journal of Chemical Physics, Vol. 150, Issue 12 https://doi.org/10.1063/1.5084248	journal	March 2019
Liquid-liquid separation of aqueous solutions: A molecular dynamics study Yagasaki, Takuma; Matsumoto, Masakazu; Tanaka, Hideki The Journal of Chemical Physics, Vol. 150, Issue 21 https://doi.org/10.1063/1.5096429	journal	June 2019
Seeding approach to bubble nucleation in superheated Lennard-Jones fluids Rosales-Pelaez, P.; Garcia-Cid, M. I.; Valeriani, C. Physical Review E, Vol. 100, Issue 5 https://doi.org/10.1103/physreve.100.052609	journal	November 2019